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DOE OSTI2022

Ice‐Nucleating Particles That Impact Clouds and Climate: Observational and Modeling Research Needs

Abstract Atmospheric ice‐nucleating particles (INPs) play a critical role in cloud freezing processes, with important implications for precipitation formation and cloud radiative properties, and thus for weather and climate. Additionally, INP emissions respond to changes in the Earth System and climate, for example, desertification, agricultural practices, and fires, and therefore may introduce climate feedbacks that are still poorly understood. As knowledge of the nature and origins of INPs has advanced, regional and global weather, climate, and Earth system models have increasingly begun to link cloud ice processes to model‐simulated aerosol abundance and types. While these recent advances are exciting, coupling cloud processes to simulated aerosol also makes cloud physics simulations increasingly susceptible to uncertainties in simulation of INPs, which are still poorly constrained by observations. Advancing the predictability of INP abundance with reasonable spatiotemporal resolution will require an increased focus on research that bridges the measurement and modeling communities. This review summarizes the current state of knowledge and identifies critical knowledge gaps from both observational and modeling perspectives. In particular, we emphasize needs in two key areas: (a) observational closure between aerosol and INP quantities and (b) skillful simulation of INPs within existing weather and climate models. We discuss the state of knowledge on various INP particle types and briefly discuss the challenges faced in understanding the cloud impacts of INPs with present‐day models. Finally, we identify priority research directions for both observations and models to improve understanding of INPs and their interactions with the Earth System.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Re-evaluating cloud chamber constraints on depositional ice growth in cirrus clouds – Part 1: Model description and sensitivity tests

Abstract. Ice growth from vapor deposition is an important process for the evolution of cirrus clouds, but the physics of depositional ice growth at the low temperatures (<235 K) characteristic of the upper troposphere and lower stratosphere is not well understood. Surface attachment kinetics, generally parameterized as a deposition coefficient αD, control ice crystal habit and also may limit growth rates in certain cases, but significant discrepancies between experimental measurements have not been satisfactorily explained. Experiments on single ice crystals have previously indicated the deposition coefficient is a function of temperature and supersaturation, consistent with growth mechanisms controlled by the crystal's surface characteristics. Here we use observations from cloud chamber experiments in the Aerosol Interactions and Dynamics in the Atmosphere (AIDA) aerosol and cloud chamber to evaluate surface kinetic models in realistic cirrus conditions. These experiments have rapidly changing temperature, pressure, and ice supersaturation such that depositional ice growth may evolve from diffusion limited to surface kinetics limited over the course of a single experiment. In Part 1, we describe the adaptation of a Lagrangian parcel model with the Diffusion Surface Kinetics Ice Crystal Evolution (DiSKICE) model (Zhang and Harrington, 2014) to the AIDA chamber experiments. We compare the observed ice water content and saturation ratios to that derived under varying assumptions for ice surface growth mechanisms for experiments simulating ice clouds between 180 and 235 K and pressures between 150 and 300 hPa. We found that both heterogeneous and homogeneous nucleation experiments at higher temperatures (>205 K) could generally be modeled consistently with either a constant deposition coefficient or the DiSKICE model assuming growth on isometric crystals via abundant surface dislocations. Lower-temperature experiments showed more significant deviations from any depositional growth model, with different ice growth rates for heterogeneous and homogeneous nucleation experiments.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

High concentrations of ice: Investigations using polarimetric radar observations combined with in situ measurements and cloud modeling (Final Report)

This DOE-funded joint project had the over-arching goal of understanding the reasons for observed size distributions of ice particles in cold clouds. Its approach involves the use of cloud models and field observations by radar and aircraft of real storms. The project addresses three major research objectives: (1) Utilize a novel polarimetric radar technique to retrieve size distributions and amounts of ice from radar data collected during the previous DOE ARM field campaigns; (2) Evaluate the results of ice microphysical retrievals using available in situ aircraft measurements and other remote sensors (e.g., vertically pointing cloud radars and wind profilers); (3) Improve the treatment of microphysical processes leading to cloud glaciation and ice multiplication in numerical cloud models. The study was performed by three research organizations: University of Oklahoma, The Hebrew University of Jerusalem, Israel, and Lund University, Sweden. The Israel and Swedish partners were funded by the sub-awards from the University of Oklahoma. Cloud modeling studies have been performed by the research teams at The Hebrew University of Jerusalem (HUJ) and Lund University to identify the origins of high concentrations of cloud ice in areas of high ice water content (HIWC). The Hebrew University Cloud Model (HUCM) with full spectral bin microphysics and the Lund University aerosol-cloud (AC) model with a hybrid bin / bulk microphysics scheme complementing HUCM were utilized for simulations. Both research teams had particular focus on secondary ice production (SIP) as one of the possible sources of enhanced ice concentration. The HUJ group suggested a novel concept of ice multiplication during droplet freezing. It is assumed that splintering and droplet fragmentation during droplet freezing takes place because of dendritic growth within a supercooled drop. The resulting simulations of SIP generated small ice in concentrations exceeding hundreds per liter similar to what was observed in the HIWC regions of the tropical storms. The Lund team explored the SIP mechanisms such as breakup of ice particles due to ice-ice collisions and ice sublimation that are expected to dominate the continental storms. They also quantified the impact of homogeneous nucleation of cloud droplets on the total number concentration of ice at very low temperatures near the tops of the clouds. Additionally, the Lund AC model is able to simulate the effect of aerosols of various types (including biological) on the cloud life cycle and the corresponding ice production. The HUCM / AC model was used to simulate one of the “golden” cases of the DOE MC3E campaign on 20 May 2011. The model output was converted into the fields of polarimetric radar variables using the polarimetric radar forward operator developed at the University of Oklahoma and compared with radar observations and in situ microphysical measurements onboard research aircraft. It was demonstrated that specific differential phase KDP is the best radar parameter to identify the HIWC areas and quantify the corresponding ice parameters. For the first time, the shape of the vertical profile of KDP was realistically reproduced by the cloud model with the KDP maximum in the dendritic growth layer (DGL) centered at the -15°C isotherm. The University of Oklahoma team has developed a methodology for polarimetric radar retrievals of such microphysical parameters of ice as ice water content (IWC), mean volume diameter (Dm), and total number concentration (Nt) of ice particles. These retrievals have been validated using in situ aircraft measurements during 6 field campaigns and proved to be quite robust and reliable. This allowed to build the first climatology of the vertical profiles of polarimetric radar variables and retrieved microphysical parameters for the three types of weather systems: continental MCSs, maritime MCSs, and tropical cyclones / hurricanes (Hu and Ryzhkov 2022). The data were collected by a multitude of the WSR-88D radars in 13 continental and 10 maritime MCSs and 11 landfalling hurricanes. The HIWC areas were identified within the examined storms and the corresponding “HIWC statistics” was compared with the “background” one without HIWC. An overarching conclusion of the study is that maritime tropical storms (MCSs and hurricanes) are characterized by smaller size ice in higher concentration compared to the continental MCSs. High ice water content in the HIWC areas is primarily caused by a strong jump in a number concentration of ice particles rather than the increase of their size compared to the “background” environment. This may point to the homogeneous nucleation of excessive amounts of supercooled droplets and / or secondary ice production as the possible origins of HIWC. Such a climatology provides a good observational reference for the modelers to evaluate the performance of their models. As an example, the in-depth analysis of the 20 May 2011 MC3E case shows that the advanced cloud models developed in the course of this study still tend to underestimate the number concentration of ice in the HIWC areas although they succeed in reproducing realistically looking vertical profiles of IWC and Nt. The results of the project research are summarized in 13 journal papers.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Application of aerosol-ice nucleating particle closure to establish the leading parameters governing ice crystal number concentration under commonly observed mixed-phase cloud conditions

This is the final technical report for DOE DE-SC0021034 award entitled “Application of aerosol-ice nucleating particle closure to establish the leading parameters governing ice crystal number concentration under commonly observed mixed-phase cloud conditions”. The overarching objective of this project was to gain a predictive understanding of the processes that lead from aerosols to ice-nucleating particles (INPs) to ice crystal number concentrations (ICNCs) in stratiform mixed-phase clouds where supercooled water droplets and ice crystals coexist, and to inform climate model parameterizations. During this four-year project we addressed the three main research goals of this objective: 1) Study the aerosol-INP link; 2) Develop an aerosol-cloud column model (AC-1D); and 3) Study the INP-ICNC link. Those activities significantly advanced our predictive understanding of how to represent INPs in could models and its implications on ice crystal number concentrations. The results have been published in five peer-reviewed publications with three more in review and preparation. It allowed for collaboration resulting in additional fourteen peer-reviewed publications that are concerned with the objective of this research project. This research has been communicated to the scientific community at national and international meetings and conferences by numerous talks, seminars, and posters including fifteen invited presentations. This project allowed training of four graduate students and one postdoctoral research associate resulting in one M.S. thesis and advancement to Ph.D. candidacy.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Sensitivity of Arctic Clouds to Ice Microphysical Processes in the NorESM2 Climate Model

Abstract Ice formation remains one of the most poorly represented microphysical processes in climate models. While primary ice production (PIP) parameterizations are known to have a large influence on the modeled cloud properties, the representation of secondary ice production (SIP) is incomplete and its corresponding impact is therefore largely unquantified. Furthermore, ice aggregation is another important process for the total cloud ice budget, which also remains largely unconstrained. In this study, we examine the impact of PIP, SIP, and ice aggregation on Arctic clouds, using the Norwegian Earth System Model, version 2 (NorESM2). Simulations with both prognostic and diagnostic PIP show that heterogeneous freezing alone cannot reproduce the observed cloud ice content. The implementation of missing SIP mechanisms (collisional breakup, drop shattering, and sublimation breakup) in NorESM2 improves the modeled ice properties, while improvements in liquid content occur only in simulations with prognostic PIP. However, results are sensitive to the description of collisional breakup. This mechanism, which dominates SIP in the examined conditions, is very sensitive to the treatment of the sublimation correction factor, a poorly constrained parameter that is included in the utilized parameterization. Finally, variations in ice aggregation treatment can also significantly impact cloud properties, mainly through their impact on collisional breakup efficiency. Overall, enhancement in ice production through the addition of SIP mechanisms and the reduction in ice aggregation (in line with radar observations of shallow Arctic clouds) result in enhanced cloud cover and decreased TOA radiation biases, compared to satellite measurements, especially during the cold months. Significance Statement Arctic clouds remain a large source of uncertainty in projections of the future climate due to the poor representation of the microphysical processes that govern their life cycle. Ice formation is among the least understood processes. While it is widely recognized that better constraints on primary ice production (PIP) are needed to improve existing parameterizations, we show that secondary ice production (SIP) and ice aggregation can have also a significant impact on ice number concentrations. Constraining ice formation through the addition of missing SIP mechanisms and reducing ice aggregation can improve the representation of the cloud macrophysical properties and enhance total cloud cover in the Arctic region, which in turn contributes to decreased TOA radiation biases in the cold months.

Meteorology & Atmospheric Sciences↗

DOE OSTI2025

Immersion Freezing in Particle-Based Aerosol-Cloud Microphysics: A Probabilistic Perspective on Singular and Time-Dependent Models

Cloud droplets containing immersed ice-nucleating particles (INPs) may freeze at temperatures above the homogeneous freezing threshold temperature in a process referred to as immersion freezing. In modeling studies, immersion freezing is often described using either so-called “singular” or “time-dependent” parameterizations. Here, we compare both approaches and discuss them in the context of probabilistic particle-based (super-droplet) cloud microphysics modeling. First, using a box model, we contrast how both parameterizations respond to idealized ambient cooling rate profiles and quantify the impact of the polydispersity of the immersed surface spectrum on the frozen fraction evolution. Presented simulations highlight that the singular approach, constituting a time-integrated form of a more general time-dependent approach, is only accurate under a limited range of ambient cooling rates. The time-dependent approach is free from this limitation. Second, using a prescribed-flow two-dimensional cloud model, we illustrate the macroscopic differences in the evolution in time of ice particle concentrations in simulations with flow regimes relevant to ambient cloud conditions. The flow-coupled aerosol-budget-resolving simulations highlight the benefits and challenges of modeling cloud condensation nuclei activation and immersion freezing on insoluble ice nuclei with super-particle methods. The challenges stem, on the one hand, from heterogeneous ice nucleation being contingent on the presence of relatively sparse immersed INPs, and on the other hand, from the need to represent a vast population of particles with relatively few so-called super particles (each representing a multiplicity of real particles). We discuss the critical role of the sampling strategy for particle attributes, including the INP size, the freezing temperature (for singular scheme) and the multiplicity.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Improving parameterization of ice microphysical processes in Arctic clouds using a synergistic modeling and observational approach (Final Report)

The primary goals of the project were to: 1) Improve the fundamental quantitative models of ice growth processes using ARM radar observations. 2) Better understand the growth of ice particle populations through vapor deposition, riming, and aggregation in Arctic clouds using a new particle-property microphysical model. 3) Robustly estimate and constrain key unknown model parameters using ARM radar observations combined with the particle-property model to develop an improved parameterization of ice growth processes for traditional bulk parameterizations used in cloud and climate models.

58 GEOSCIENCES↗

DOE OSTI2023

A 1D Model for Nucleation of Ice From Aerosol Particles: An Application to a Mixed‐Phase Arctic Stratus Cloud Layer

Abstract Mixed‐phase clouds (MPCs) have been identified as significant contributors to uncertainties in climate projections, attributable to model representation of processes controlling the formation and loss of supercooled water droplets and ice particles from the atmosphere. Arctic MPCs are commonly widespread and long‐lived, with sustained ice crystal formation processes that challenge current understanding. This study examines the ice‐nucleating particle (INP) reservoir dynamics governing immersion‐mode heterogeneous freezing in an observed case of Arctic MPCs using a simplified 1D aerosol‐cloud model. The model setup includes prescribed dynamical forcings and thermodynamic profiles, and represents INPs as multicomponent and polydisperse particle size distributions. Diagnostic and prognostic approaches to immersion freezing parameterization are compared, including time‐independent (singular) number‐ and surface area‐based descriptions and a time‐dependent description following classical nucleation theory (CNT). The choice of freezing parameterization defines the size of the INP reservoir. The CNT‐based description yields an orders of magnitude larger INP reservoir than the singular parameterizations, which is the dominant factor for sustained ice crystal formation. The efficiency of the freezing process and cloud cooling are of secondary importance. A diagnostic treatment neglecting INP loss is only accurate when the INP reservoir size is large and INP depletion weak. Since a larger INP reservoir sustains ice crystal formation substantially longer, and ice water path scales with ice crystal concentrations for the conditions considered, resolving the source of differences in INP reservoir dynamics due to model implementation is a high priority for advancing climate model physics.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

A Refined Understanding of the Ice Cloud Longwave Scattering Effects in Climate Model

Abstract Because longwave (LW) absorption by greenhouse gases and clouds is more significant than the LW scattering effect by clouds, most climate models neglect cloud LW scattering to save computational costs. Ignoring cloud LW scattering directly overestimates outgoing longwave radiation (OLR). This study included ice‐cloud LW scattering treatment in the Exascale Energy Earth System Model (E3SM) version 2 and ran fully‐coupled simulations, prescribed sea surface temperature simulations, and offline radiative transfer calculations to comprehensively assess the impact of ice‐cloud LW scattering on global climate simulation. The instantaneous effect due to ice‐cloud LW scattering reduces the OLR by ∼1 W/m 2 on the global average and 2 W/m 2 on the tropical average. Tropospheric warming and high cloud amount reduction act to partially compensate for such instantaneous OLR reduction caused by the inclusion of LW scattering. When the simulation reaches the equilibrium, the surface warms by 0.66 K on average with respect to the simulation without LW scattering, with the Arctic surface temperature differences more than twice as large as that of the global mean. The impact of including LW scattering on the simulated climate change in response to 4 × CO 2 is also assessed. While including the cloud LW scattering does not significantly modify radiative forcing and total radiative feedback under such a scenario, it results in a 10% more positive cloud feedback.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Vertical Structure and Ice Production Processes of Shallow Convective Postfrontal Clouds over the Southern Ocean in MARCUS. Part II: Modeling Study

Abstract Part I of this series presented a detailed overview of postfrontal mixed-phase clouds observed during the Measurements of Aerosols, Radiation, and Clouds over the Southern Ocean (MARCUS) field campaign. In Part II, we focus on a multiday (23–26 February 2018) case with the aim of understanding ice production as well as model sensitivity to ice process parameterizations using the Weather Research and Forecasting (WRF) Model. The control simulation with the Predicted Particle Properties (P3) microphysics scheme underestimates the ice content and overestimates the supercooled liquid water content, contrary to the bias common in global climate models. The simulations targeted at ice production processes show negligible sensitivity to cloud droplet number concentrations. Further, neither increasing ice nuclei particle (INP) concentrations to an unrealistic level nor adjusting it to MARCUS field estimations alone guarantees more ice production in the model. However, the simulated clouds are found to be highly sensitive to the implementation of immersion freezing, the thresholding of condensation/deposition freezing initiation, and the rime splintering process. By increasing immersion freezing of cloud droplets, relaxing thresholds for condensation/deposition freezing, or removing rime splintering thresholds, the model significantly improves its performance in producing ice. The relaxation of the immersion freezing temperature threshold to the observed cloud-top temperature suggests an in-cloud seeder–feeder mechanism. The results of this work call for an increase in observations of INP, especially over the remote Southern Ocean and at relatively high temperatures, and measurements of ice particle size distributions to better constrain ice nucleating processes in models.

Meteorology & Atmospheric Sciences↗

DOE OSTI2024

Cloud-Resolving ICON Simulations of Secondary Ice Production in Arctic Mixed-Phase Stratocumuli Observed during M-PACE

Field measurements and modeling studies suggest that secondary ice production (SIP) may close the gap between observed Arctic ice nucleating particle (INP) concentrations and ice crystal number concentrations ni. Here, we explore sensitivities with respect to the complexity of different INP parameterizations under the premise that ni is governed by SIP. Idealized, cloud-resolving simulations are performed for the marine cold air outbreak cloud deck sampled during the Mixed-Phase Arctic Cloud Experiment (M-PACE) with the Icosahedral Nonhydrostatic (ICON) model. The impact of the droplet shattering (DS) of raindrops and collisional breakup (BR) in addition to the existing Hallet–Mossop rime splintering mechanism were investigated. Overall, 12 different model experiments (12-h runs) were performed and analyzed. Despite the considerable amount of uncertainty remaining with regard to SIP mechanisms and their process representation in numerical models, we conclude from these experiments that (i) only simulations where DS dominates the SIP signal (potentially amplified by BR) capture observed ice-phase and liquid-phase cloud properties, and (ii) SIP events cluster around the convective outflow region and are structurally linked to mesoscale cloud organization. In addition, interactions with primary nucleation parameterizations of varied complexity were investigated. Here, our simulations show that (i) a stable long-lived mixed-phase cloud (MPC) can be maintained in the absence of primary nucleation once SIP is established, (ii) experiments using a computationally more efficient relaxation-based parameterization of primary nucleation are statistically invariant from simulations considering prognostic INP, and (iii) primary nucleation at cloud-top controls the areal extent of the mixed-phase cloud region, and reduces SIP efficacy via DS due to increased depletion of cloud liquid throughout the entire cloud column.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Development of a triple-moment ice-phase cloud microphysics scheme and its application to the Single Column Atmosphere Model

Parameterization of cloud microphysics is critical for accurate simulation of weather and climate, in which the characteristics of cloud particle spectrum inevitably further affect climate simulation by changing the cloud evolution and cloud radiation effects. The popular currently used double-moment cloud microphysics schemes in numerical models can predict the intercept (N 0 ) and slope (λ) parameters of cloud particle spectrum but cannot predict the spectral shape parameter (μ), which hinders accurate description of cloud physical processes in climate models. Therefore, in the present study, we built upon the ideas of previously developed triple-moment cloud microphysics scheme, considered radar reflectivity factor as the third predictor in addition to number and mass concentration, and introduced its related prediction equation to the Single Column Atmosphere Model Version 5.3 (SCAM5.3). Moreover, the relevant microphysical process formulas in the model were revised, and a triple-moment ice-cloud microphysics scheme was constructed to predict the μ of ice particle spectrum. Based on this model, a 29-day case of the Atmospheric Radiation Measurement Program in the summer of 1997 (ARM97) was simulated, and the differences in cloud fraction and radiation simulations between the double- and triple-moment schemes were analysed. The μ of ice particle spectrum predicted by the triple-moment scheme mainly ranged from 0 to 4; the peak value was around 2, and at least 85% of the μ values were greater than the default 0. Therefore, the μ=0 setting in the double-moment scheme is unreasonable. Moreover, the developed triple-moment ice-cloud microphysics scheme yielded a narrower ice particle spectrum, which was closer to the observation results of previous studies, than the double-moment cloud microphysics scheme (e.g., height=233 hPa). Furthermore, compared with the double-moment scheme, the triple-moment scheme achieved closer simulations of the cloud fraction observations, particularly for ice clouds in the upper levels. Considering the close association between cloud fraction and radiation, the error with the triple-moment scheme was smaller than that with the double-moment scheme regardless of the shortwave (surface downward shortwave radiation, net downward shortwave radiation at the top of the atmosphere, and net shortwave radiation at the surface) or longwave (surface downward longwave radiation and net longwave radiation at the surface) flux density. Finally, the improvement mechanism of the triple-moment scheme on cloud fraction and radiation simulations was explored. The major reason is that the triple-moment scheme weakens the autoconversion of ice crystal to form snow and enhances the growth process of ice crystal deposition, thereby increasing the mass concentration of ice crystals and ice cloud fraction. Overall, the developed triple-moment ice-cloud microphysics scheme can help improve the simulation ability of models for cloud-climate feedback and other processes.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Developing and Testing a Novel Stochastic Ice Microphysics Parameterization for Cloud and Climate Models Using ARM Field Campaign Data (Final Progress Report)

The major goals of this project were: 1) to use field campaign measurements from DOE’s Atmospheric Radiation Measurement (ARM) program to characterize variability of important parameters describing properties of ice particles in the atmosphere; 2) based on this observational analysis, to develop a parameterization scheme for weather and climate models that stochastically varies these parameters, and implement the new scheme into a weather model called the Weather Research and Forecasting model (WRF); 3) to use WRF coupled with the new stochastic scheme to simulate ARM field campaign thunderstorm cases and analyze how accounting for this parameter variability affects the model simulations. This work was performed jointly between the National Center for Atmospheric Research, University of Oklahoma, and University of Utah. To accomplish these goals, we extended an approach previously developed to characterize the variability in the size distribution of ice particles to parameters that are explicitly represented in models (i.e., relationships between ice particle mass and size, and between particle fall velocity and size). Our project was, to our knowledge, the first to apply observationally-constrained estimates of this parameter variability describing mass-size and fall velocity-size in a modeling framework. Our results showed efficacy of the approach, evaluated using ARM observations. Similarly, to our knowledge, work in this project was the first to propose and evaluate in detail a stochastic approach for unresolved turbulent mixing in high-resolution model simulations against detailed, benchmark large eddy simulations and ARM observations. Results showed some promising behavior, particularly with increased mixing and dilution of air in thunderstorm cores with surrounding environmental air, bringing the stochastic simulations closer to the benchmark large eddy simulations; however, results were somewhat degraded using stochastic mixing compared to observations from the AMIE/DYNAMO field campaign. This project also further refined and applied a modeling methodology called “piggybacking” that can robustly separate dynamical and thermodynamic impacts of model changes, and comparison studies of different models based on cases developed from ARM observations. Finally, this project directly supported three graduate students who completed their PhDs as well as a postdoctoral research fellow.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

A Comparative Study of Cloud Properties Between Northern and Southern High Latitudes Based on ARM Observations and EAMv2 Simulations

Earth's high-latitude regions show a considerable amount of cloud coverage, which significantly affects global radiation budgets. Here, in this study, we examine ground- and ship-based remote sensing observations from two Atmospheric Radiation Measurement (ARM) field campaigns conducted in the high-latitude regions of Northern and Southern Hemispheres (NH and SH). A comparison of macrophysical properties for low, mid-level, high, and deep clouds shows that the cloud top heights and thickness values are higher in the Arctic for each cloud type compared with the Southern Ocean and Antarctic regions, possibly due to higher sea surface temperatures in the north Atlantic. The Arctic also shows lower ice phase occurrence frequencies compared with the SH high latitudes for low clouds. For high, mid-level and deep clouds, the cloud phase distributions as a function of temperature show small geographical variabilities. The observations are then compared with the Department of Energy (DOE) Energy Exascale Earth System Model (E3SM) to evaluate the representations of these cloud properties. Here, the results show that the model captures cloud base and top heights well and reproduces the differences in cloud macrophysical properties between the two hemispheres. But the model underestimates ice phase frequencies for all cloud types. Such model cloud phase bias is strongly correlated with positive relative humidity biases and negative aerosol number concentration biases, indicating an important role of relative humidity and aerosols in modulating cloud phase partitioning in the model.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Advancing the Understanding of Cloud Microphysical Processes and Aerosol Indirect Effects in High-Latitude Mixed-Phase Clouds by Linking ARM Measurements with Climate Model Simulations (Final Report)

The key objectives of this project were to advance our understanding of cloud microphysical characteristics and aerosol indirect effects on mixed-phase clouds in high latitudes. To improve the representation of ice and mixed-phase clouds in Earth System Models (ESMs), we propose an integrated observation and modeling study of cloud macro- and microphysical properties, including spatial heterogeneities, mass partitioning between ice crystals and supercooled liquid water, effects of ice nucleating particles (INPs), and efficiency of secondary ice production (SIP), etc. Specifically, we took four main approaches in this project: (1) examining macro- and microphysical properties of ice and mixed-phase clouds based on in-situ and ground-based observations from multiple field campaigns funded by the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) program, including the Mixed-Phase Arctic Cloud Experiment (M-PACE), Indirect and Semi-Direct Aerosol Campaign (ISDAC), Ice Nucleating Particle Sources at Oliktok Point (INPOP), ARM West Antarctic Radiation Experiment (AWARE), Measurements of Aerosols, Radiation, and Clouds over the Southern Ocean (MARCUS), and Macquarie Island Cloud and Radiation Experiment (MICRE); (2) evaluating the DOE Energy Exascale Earth System Model (E3SM) simulations based on observations, particularly for ice and mixed-phase cloud microphysical properties; (3) examining the impacts of INPs on ice and mixed-phase clouds. Specifically, a series of comparisons were conducted using observations over the Arctic, Southern Ocean, and Antarctica, including comparisons between the lower and higher southern latitudes as well as comparisons between the northern and southern hemispheres. In addition, aerosol indirect effects from distinct sources of dust particles were examined; and (4) investigating the impacts of SIP. Ultimately, these results helped to improve cloud microphysics and aerosol-cloud interaction parameterizations in the E3SM model. Overall, the project provided improved understanding regarding various factors, including thermodynamic, dynamic, and aerosol conditions, on the micro- and macrophysical properties of ice and mixed-phase clouds in the high latitudes. Resulting analysis helped to provide an improved physical basis for refining the current cloud microphysics parameterizations related to ice and mixed-phase clouds in E3SM.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Ship-based Observations and Climate Model Simulations of Cloud Phase over the Southern Ocean

The Southern Ocean (SO) clouds exert a significant influence on the Earth’s radiation budget. Here we analyzed ship-based remote sensing observations of SO clouds over a five-month long DOE ARM Measurements of Aerosols, Radiation and Clouds over the Southern Oceans (MARCUS) field campaign to better understand cloud phase variability. We developed a method to classify eight categories of hydrometeors (ice, liquid, mixed phase, rain, drizzle, snow, aerosols, and clear sky) based on measurements of lidar, radar and radiosondes. Cloud thermodynamic phases (liquid, ice and mixed phase) at coarser scales were further derived to compare with the DOE Energy Exascale Earth System Model version 1 (E3SMv1) simulation and the Earth Model Column Collaboratory (EMC 2 ) instrument simulator. For a scale-aware comparison with climate model simulations, we found that spatially averaging the raw remote sensing data (e.g., backscatter, reflectivity) results in increased cloud cover and cloud liquid, whereas, directly averaging cloud phase from higher to lower resolution maintains clear air regions and is thus recommended for in-cloud frequency comparisons. For cloud thermodynamic phases in stratiform clouds, the E3SM underestimates cloud ice and overestimates cloud liquid at temperatures between -40 and 0°C. When latitudes increase, both observations and simulations show a transition of dominant phase from liquid to ice for cloud tops as well as for the entire cloud columns, but the model underestimation of ice phase is more severe at higher latitudes. Such model bias is unlikely caused by spatial scale differences or lack of heterogeneity in cloud vertical structure in the simulation.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Important ice processes are missed by the Community Earth System Model (CESM) in Southern Ocean mixed–phase clouds: Bridging SOCRATES observations to model developments

Global climate models (GCMs) are challenged by difficulties in simulating cloud phase and cloud radiative effect over the Southern Ocean (SO). Some of the new generation GCMs predict too much liquid and too little ice in mixed-phase clouds. This misrepresentation of cloud phase in GCMs results in weaker negative cloud feedback over the SO and a higher climate sensitivity. Based on a model comparison with observational data obtained during the Southern Ocean Cloud Radiation and Aerosol Transport Experimental Study (SOCRATES), this study addresses a key uncertainty in the Community Earth System Model version 2 (CESM2) related to cloud phase, namely ice formation in pristine remote SO clouds. It is found that sea spray organic aerosols (SSOA) are the most important type of ice nucleating particles (INPs) over the SO with concentrations one order of magnitude higher than those of dust INPs based on measurements and CESM2 simulations. Secondary ice production (SIP) which includes riming splintering, rain droplet shattering, and ice-ice collisional fragmentation as implemented in CESM2 is the dominant ice production process in moderately cold clouds with cloud temperatures greater than –20°C. SIP enhances the in-cloud ice number concentrations (Ni) by 1-3 orders of magnitude and predicts more mixed-phase (with percentage occurrence increased from 15% to 21%), in better agreement with the observations. Finally, this study highlights the importance of accurately representing cloud phase over the pristine remote SO by considering the ice nucleation of SSOA and SIP processes, which are currently missing in most GCM cloud microphysics parameterizations.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Climatology of the Vertical Profiles of Polarimetric Radar Variables and Retrieved Microphysical Parameters in Continental/Tropical MCSs and Landfalling Hurricanes

Most existing cloud models tend to overestimate the size of cloud ice particles and underestimate their concentration. This emphasizes the need to provide a reliable observational reference to optimize cloud model performance, particularly in areas of high concentration of ice at high altitudes. The dual-polarization radars give the community a unique opportunity to quantify cloud ice with a good accuracy using polarimetric radar retrievals. Here, in this study, we utilize the network of operational WSR-88D radars to build a climatology of the vertical profiles of radar variables, such as radar reflectivity Z, differential reflectivity Z DR , and specific differential phase K DP as well as the radar-retrieved vertical profiles of ice water content (IWC) above the melting layer and liquid water content below it, mean volume diameter D m , and total number concentration N t of ice and liquid particles. Such climatology was created for continental/marine mesoscale convective systems (MCSs) and tropical cyclones including hurricanes. The dataset includes 13 continental MCSs, 10 marine MCSs, and 11 tropical cyclones. Separate statistics of the “background” vertical profiles and the ones associated with high IWC aloft have been obtained in the course of this study. It is shown that continental MCSs exhibit larger size of ice in lower concentration aloft compared to the marine MCSs and especially tropical cyclones/hurricanes. A combination of high KDP and low Z aloft signifies lower D m , higher N t , and often substantial IWC.

54 ENVIRONMENTAL SCIENCES↗